用HPLC 分离和鉴定大气中的羰基化合物

大气中的挥发性羰基化合物可以通过2,4-二硝基苯肼(DNPH)原位衍生化而被捕集.采用反相HPLC 可以洗脱和分析这些羰基衍生物.本文采用该方法监测了美国佛蒙特州大气样品中的痕量甲醛、乙醛和丙酮.     

Fish mercury increase in Lago Manso, a new hydroelectric reservoir in tropical Brazil

It has been frequently demonstrated that mercury (Hg) concentrations in fish rise in newly constructed hydroelectric reservoirs in the Northern Hemisphere. In the present work, we studied whether similar effects take place also in a tropical upland reservoir during impoundment and discuss possible causes and implications. Total Hg concentrations in fish and several soil and water parameters were determined before and after flooding at Rio Manso hydroelectric power plant in western Brazil. The Hg concentrations in soil and sediment were within the background levels in the region (22-35 ng g(-1) dry weight). There was a strong positive correlation between Hg and carbon and sulphur in sediment. Predatory fish had total Hg concentrations ranging between 70 and 210 ng g(-1) f.w. 7 years before flooding and between 72 and 755 ng g(-1) f.w. during flooding, but increased to between 216 and 938 ng g(-1) f.w. in the piscivorous and carnivorous species Pseudoplatystoma fasciatum, cachara, and Salminus brasiliensis, dourado, 3 years after flooding. At the same time, concentrations of organic carbon in the water increased and oxygen concentrations decreased, indicating increased decomposition and anoxia as contributing to the increased Hg concentrations in fish. The present fish Hg concentrations in commonly consumed piscivorous species are a threat to the health of the population dependent on fishing in the dam and downstream river for sustenance. Mercury exposure can be reduced by following fish consumption recommendations until fish Hg concentrations decrease to a safe level.     

Changes in soil characteristics and plant species composition along a moisture gradient in a Mediterranean pasture

Soil physicochemical characteristics, total aboveground biomass, number of species and relative abundance of groups and individual species were measured along a moisture gradient in a pasture, flooded in part during winter through early summer, adjacent to Pamvotis lake in Ioannina, Greece. Soil and vegetation measurements were conducted in 39 quadrats arranged in four zones perpendicular to the moisture gradient. The zone closest to the lake, recently separated from the lake, became part of the pasture and its soil texture was quite different from that of the other zones with a substrate containing 91% sand. Except for pH, this zone had the lowest values in the other five soil physicochemical characteristics measured (organic matter, total and extracted inorganic nitrogen, Olsen extracted phosphorus and extractable potassium); in the other zones organic matter, total nitrogen, phosphorus and potassium tended to increase from the driest to the wettest zone. Total aboveground biomass, ranging from 280 to 840 gm-2, is high for herbaceous pastures in the conditions of Mediterranean climate and it was not related to distance from the lake's shoreline, although the highest values were measured at intermediate distances, or to any of the various soil characteristics measured. Also, the number of species/0.25 m2 was not related to any of the various soil characteristics, but it was highest at the intermediate distances from the lake's shoreline. Species composition varied along the moisture gradient. Forbs as well as annual grasses and legumes declined in abundance from the driest to the wettest places; the reverse was the case for sedges and perennial grasses and legumes. These results indicate that the soil moisture gradient was the principal factor affecting soil characteristics and plant species composition. Since most species were recorded in all the four zones of the pasture, indicating that these can tolerate all variations in abiotic conditions of pasture, the vegetation zonation seems to be influenced by competition. Each functional group of species tends to dominate in a particular range of the soil moisture gradient where it is better suited and tends to exclude competitively other species. Management practices (mowing and grazing) affect the kinds of processes which maintain the observed community structure either by preventing the establishment of later successional species, like reeds and woody species, or by moderating the shoot competition, especially in the wetter zones, and thus permitting the creeping species to grow successfully.     

Impacts of land cover on stream hydrology in the West Georgia Piedmont, USA

The southeastern United States is experiencing rapid urban development. Consequently, Georgia's streams are experiencing hydrologic alterations from extensive development and from other land use activities such as livestock grazing and silviculture. A study was performed to assess stream hydrology within 18 watersheds ranging from 500 to 2500 ha. Study streams were first, second, or third order and hydrology was continuously monitored from 29 July 2003 to 23 September 2004 using InSitu pressure transducers. Rating curves between stream stage (i.e., water depth) and discharge were developed for each stream by correlating biweekly discharge measurements and stage data. Dependent variables were calculated from discharge data and placed into 4 categories: flow frequency (i.e., the number of times a predetermined discharge threshold is exceeded), flow magnitude (i.e., maximum and minimum flows), flow duration (i.e., the amount of time discharge was above or below a predetermined threshold), and flow predictability and flashiness. Fine resolution data (i.e., 15-min interval) were also compared to daily discharge data to determine if resolution affected how streams were classified hydrologically. Urban watersheds experienced flashy discharges during storm events, whereas pastoral and forested watersheds showed less flashy hydrographs. Also, in comparison to all other flow variables, flow frequency measures were most strongly correlated to land cover. Furthermore, the stream hydrology was explained similarly with both the 15-min and daily data resolutions.     

Diuron in surface runoff and tile drainage from two grass-seed fields

The typical method of cool-season grass-seed production in Mediterranean climates briefly exposes surface waters to potentially high concentrations of the herbicide diuron [3-(3,4-dichlorophenyl)-1,1-dimethyl urea] during the initial season of growth. To better understand the process, and the degree, of diuron transport from agricultural fields, two grass-seed fields in the Willamette Valley of Oregon were monitored for diuron loss in surface runoff and tile drainage during the first wet season after planting. Initial diuron concentrations in surface runoff were high (>1000 microg L(-1) in one field and >100 microg L(-1) in the other), though they decreased by two orders of magnitude by the end of the season. Concentrations in the tile drains were as much as 1000 times lower than in the surface runoff during the first few weeks of runoff events, and they remained lower than surface water concentrations throughout the season. Total losses in surface runoff were between 1.3 and 3% of the amount applied-much higher than losses via the tile drains. It is also shown by means of a simple first-order decay model that, when little information is available, it may be best to describe diuron depletion in runoff water as a function of cumulative rainfall during the wet season.     

Temporal and spatial distributions of sediment total organic carbon in an estuary river

Understanding temporal and spatial distributions of naturally occurring total organic carbon (TOC) in sediments is critical because TOC is an important feature of surface water quality. This study investigated temporal and spatial distributions of sediment TOC and its relationships to sediment contaminants in the Cedar and Ortega Rivers, Florida, USA, using three-dimensional kriging analysis and field measurement. Analysis of field data showed that large temporal changes in sediment TOC concentrations occurred in the rivers, which reflected changes in the characteristics and magnitude of inputs into the rivers during approximately the last 100 yr. The average concentration of TOC in sediments from the Cedar and Ortega Rivers was 12.7% with a maximum of 22.6% and a minimum of 2.3%. In general, more TOC accumulated at the upper 1.0 m of the sediment in the southern part of the Ortega River although the TOC sedimentation varied with locations and depths. In contrast, high concentrations of sediment contaminants, that is, total polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs), were found in sediments from the Cedar River. There was no correlation between TOC and PAHs or PCBs in these river sediments. This finding is in contradiction to some other studies which reported that the sorption of hydrocarbons is highly related to the organic matter content of sediments. This discrepancy occurred because of the differences in TOC and hydrocarbon source input locations. It was found that more TOC loaded into the southern part of the Ortega River, while almost all of the hydrocarbons entered into the Cedar River. This study suggested that the locations of their input sources as well as the land use patterns should also be considered when relating hydrocarbons to sediment TOC.     

Performance characteristics of sequential separation and quantification of lead-210 and polonium-210 by ion exchange chromatography and nuclear spectrometric measurements

A selective separation and quantitative determination procedure for 210Pb and 210Po in various environmental matrices from different sources such as IAEA-326 soil, phosphate rocks (PR), and phosphogypsum (PG) was developed. The tested samples were digested sequentially using concentrated mineral acids (HF, HNO3) by a programmable high-pressure microwave digestion system. The sample solution was loaded onto a preconditioned ion exchange column (Sr-resin) for chromatographic separation. Polonium-210 was eluted by 6 M HNO3 then spontaneously deposited onto polished silver discs to be measured using low-background alpha spectrometry. Lead-210 was sequentially eluted using 6 M HCl solution, precipitated as lead oxalate, dissolved in HNO3 solution, and mixed with scintillation cocktail to be measured by liquid scintillation counting (LSC). Performance of the developed procedure was tested using a reference soil (IAEA-326), with recommended isotope values, that was used as a quality control to assess separation and quantification efficiency (recovery %). The minimum detectable activities of 210Pb and 210Po were found to be 24 and 0.28 Bq kg(-1) for the measurements using LSC and alpha spectrometry, respectively. The recoveries (%) of 210Pb and 210Po were found to be 80 and 60%, respectively. To test the validity of the proposed LSC method, a comparative study was performed by measuring 210Pb activity concentration in test samples by nondestructive gamma-ray spectrometry.     

Increased wind erosion from forest wildfire: implications for contaminant-related risks

Assessments of contaminant-related human and ecological risk require estimation of transport rates, but few data exist on wind-driven transport rates in nonagricultural systems, particularly in response to ecosystem disturbances such as forest wildfire and also relative to water-driven transport. The Cerro Grande wildfire in May of 2000 burned across ponderosa pine (Pinus ponderosa Douglas ex P.&C. Lawson var. scopulorum Englem.) forest within Los Alamos National Laboratory in northern New Mexico, where contaminant transport and associated post-fire inhalation risks are of concern. In response, the objectives of this study were to measure and compare wind-driven horizontal and vertical dust fluxes, metrics of transport related to wind erosion, for 3 yr for sites differentially affected by the Cerro Grande wildfire: unburned, moderately burned (fire mostly confined to ground vegetation), and severely burned (crown fire). Wind-driven dust flux was significantly greater in both types of burned areas relative to unburned areas, by more than one order of magnitude initially and by two to three times 1 yr after the fire. Unexpectedly, the elevated dust fluxes did not decrease during the second and third years in burned areas, apparently because ongoing drought delayed post-fire recovery. Our estimates enable assessment of amplification in contaminant-related risks following a major type of disturbance-wildfire, which is expected to increase in intensity and frequency due to climate change. More generally, our results highlight the importance of considering wind- as well as water-driven transport and erosion, particularly following disturbance, for ecosystem biogeochemistry in general and human and ecological risk assessment in particular.     

Distance and flow effects on microsphere transport in a large gravel column

Consumption of microbially contaminated ground water can cause adverse health effects and the processes involved in pathogen transport in aquifers need to be understood. The influences of distance, flow velocity, and colloid size on colloid transport were examined in homogenous pea-gravel media using an 8-m column and three sizes (1, 5, and 10 microm) of microspheres. Experiments were conducted at three flow rates by simultaneously injecting microspheres with a conservative tracer, bromide. Observed concentrations were simulated with CXTFIT and analyzed with filtration theory. The results demonstrate that colloid concentration is strongly log-linearly related to transport distance (as suggested by filtration theory) in coarse gravels, similar to our previous field studies. In contrast, the log-linear relationship is often reported to be invalid in fine porous media. The observed log-linear relationship is possibly because straining is negligible in the coarse gravels investigated. This has implications in predicting setback distances for land disposal of effluent, and suggests that setback distances in gravel aquifers can be estimated using constant spatial removal rates (f). There was an inverse relationship between transport distance and colloidal concentration, but not with temporal attachment rate (katt) and collision coefficient (alpha). Increases in flow velocity result in increasing colloidal recovery, katt and alpha but decreasing f. Increases in sphere size result in decreasing colloidal recovery with increasing katt, f, alpha, and velocity enhancement. Diffusion is the dominant collision mechanism for 1-microm spheres (81-88%), while settling dominates for 5- and 10-microm spheres (> 87%), and interception is very small for all spheres investigated.     

Iron and arsenic release from aquifer solids in response to biostimulation

Biostimulation has been used at various contaminated sites to promote the reductive dechlorination of trichloroethylene (TCE), but the addition of carbon and energy donor also stimulates bacteria that use Fe(III) as the terminal electron acceptor (TEA) in potential competition with dechlorination processes. Microcosm studies were conducted to determine the influence of various carbon donors on the extent of reductive dissolution of aquifer solids containing Fe(III) and arsenic. Glucose, a fermentable and respirable carbon donor, led to the production of 1500 mg Fe(II) kg(-1), or 24% of the total Fe in the aquifer sediment being reduced to Fe(II), whereas the same concentration of carbon as acetate resulted in only 300 mg Fe(II) kg(-1) being produced. The biogenic Fe(II) produced with acetate was exclusively associated with the solid phase whereas with fermentable carbon donors as whey and glucose, 22 and 54% of the Fe(II) was in solution. With fermentation, some of the metabolites appear to be electron shuttling chemicals and chelating agents that facilitate the reductive dissolution of even crystalline Fe(III) oxides. Without the presence of electron shuttling chemicals, only surficial Fe in direct contact with the bacteria was bioavailable, as illustrated when acetate was used. Regardless of carbon donor type and concentration, As concentrations in the water exceeded drinking water standards. The As dissolution appears to have been the result of the direct use of As as an electron acceptor by dissimilatory arsenic reducing bacteria. Our findings indicate that selection of the carbon and energy donor for biostimulation for remediation of chlorinated solvent impacted aquifers may greatly influence the extent of the reductive dissolution of iron minerals in direct competition with dechlorination processes. Biostimulation may also result in a significant release of As to the solution phase, contributing to further contamination of the aquifer.